Higher-order triplet interaction in energy-level modeling of excited-state absorption for an expanded porphyrin cadmium complex

Michael M. McKerns; Wenfang Sun; Chris M. Lawson; Gary M. Gray

doi:10.1364/JOSAB.22.000852

Higher-order triplet interaction in energy-level modeling of excited-state absorption for an expanded porphyrin cadmium complex

Michael M. McKerns, Wenfang Sun, Chris M. Lawson, and Gary M. Gray

Journal of the Optical Society of America B
Vol. 22,
Issue 4,
pp. 852-861
(2005)
•https://doi.org/10.1364/JOSAB.22.000852

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Michael M. McKerns, Wenfang Sun, Chris M. Lawson, and Gary M. Gray, "Higher-order triplet interaction in energy-level modeling of excited-state absorption for an expanded porphyrin cadmium complex," J. Opt. Soc. Am. B 22, 852-861 (2005)

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Previously assigned OCIS codes
- Nonlinear optical materials (160.4330)
- Organic materials (160.4890)
- Transition-metal-doped materials (160.6990)
- Nonlinear optics (190.0190)
- Nonlinear optics, materials (190.4400)

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Abstract

Recent measurements of transmission versus fluence for a methanol-solvated asymmetric pentaazadentate porphyrin-like (APPC) cadmium complex, $[(C_{6} H_{4} - APPC) Cd] Cl,$ showed the limitations of current energy-level models in predicting the transmission behavior of organic reverse saturable absorbers at fluences greater than 1 J/cm². A new model has been developed that incorporates higher-order triplet processes and accurately fits both nanosecond and picosecond transmission-versus-fluence data. This model has provided the first known determination of a higher triplet excited-state absorption cross section and lifetime for an APPC complex and also described a previously unreported feature in the transmission-versus-fluence data. The intersystem crossing rate and the previously neglected higher triplet excited-state absorption cross section are shown to govern the excited-state population dynamics of methanol-solvated $[(C_{6} H_{4} - APPC) Cd] Cl$ most strongly at more-practical device energies.

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Cross Section	Value (cm²)
$σ_{01}$	$8.8 \times 10^{- 18}$ a
$σ_{35}$	$2.0 \times 10^{- 17}$
$σ_{56}$	$2.8 \times 10^{- 16}$
$σ_{12}$	$3.1 \times 10^{- 17}$
$σ_{24}$	$⩽ 1.0 \times 10^{- 19}$

Decay Rate	Value (s^-1)
$k_{10}$	$2.6 \times 10^{8}$ a
$k_{13}$	$2.6 \times 10^{9}$ a
$k_{30}$	$5.6 \times 10^{4}$ b
$k_{21}$	$5.0 \times 10^{11}$
$k_{53}$	$1.2 \times 10^{11}$

Cross Section	Value (cm²)
$σ_{01}$	$8.8 \times 10^{- 18}$ a
$σ_{35}$	$2.0 \times 10^{- 17}$
$σ_{56}$	$2.8 \times 10^{- 16}$
$σ_{12}$	$3.1 \times 10^{- 17}$
$σ_{24}$	$⩽ 1.0 \times 10^{- 19}$

Decay Rate	Value (s^-1)
$k_{10}$	$2.6 \times 10^{8}$ a
$k_{13}$	$2.6 \times 10^{9}$ a
$k_{30}$	$5.6 \times 10^{4}$ b
$k_{21}$	$5.0 \times 10^{11}$
$k_{53}$	$1.2 \times 10^{11}$

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Figures (8)

Tables (2)

Equations (9)

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